Mechanistic modeling of solar photo-Fenton process with Fe3+-EDDS at neutral pH

Soriano-Molina, P.; Sánchez, José Francisco Fernandez; Alfano, Orlando Mario; Conte, Leandro; Malato, S.; Pérez, J.A. Sánchez

doi:10.1016/j.apcatb.2018.04.005

Cited by 56 publications

(22 citation statements)

References 45 publications

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“…Mailhot and co-workers introduced for the first time EDDS in Fenton and photo-Fenton processes (Huang et al, 2012(Huang et al, , 2013Li et al, 2010;Wu et al, 2014). Since then, only some few works have explored the degradation of organic micropollutants by Fe(III)-EDDS-assisted photo-Fenton (Papoutsakis et al, 2015) and solar photo-Fenton (Soriano-Molina et al, 2018, 2019Cuervo Lumbaque et al, 2019). It has been demonstrated that photo-Fenton-like reaction (5) exhibits a much higher quantum yield than conventional photo-Fenton reaction (2): 0.017 for the latter at 360 nm (Safarzadeh-Amiri et al, 1997) versus 0.10 for the former at 290-400 nm (Wu et al, 2014).…”

Section: Introductionmentioning

confidence: 99%

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

Brillas

Centellas

et al. 2020

Water Research

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This work reports the first investigation on the use of EDDS as chelating agent in photoelectro-Fenton (PEF) treatment of water at near-neutral pH. As a case study, the removal of the antidepressant fluoxetine was optimized, using an electrochemical cell composed of an IrO2-based anode an air-diffusion cathode for in-situ H2O2 production. Electrolytic trials at constant current were made in ultrapure water with different electrolytes, as well as in urban wastewater (secondary effluent) at pH 7.2. PEF with Fe(III)-EDDS (1:1) complex as catalyst outperformed electro-Fenton and PEF processes with uncomplexed Fe(II) or Fe(III). This can be explained by: (i) the larger solubilization of iron ions during the trials, favoring the production of • OH from Fenton-like reactions between H2O2 and Fe(II)-EDDS or Fe(III)-EDDS, and (ii) the occurrence of Fe(II) regeneration from Fe(III)-EDDS photoreduction, which was more efficient than conventional photo-Fenton reaction with uncomplexed Fe(III). The greatest drug concentration decays were achieved at low pH, using only 0.10 mM Fe(III)-EDDS in a 1:1 molar ratio, although complete removal in wastewater was feasible only with 0.20 mM Fe(III)-EDDS due to the greater formation of • OH. The effect of the applied current and anode nature was rather insignificant. A progressive destruction of the catalytic complex was unveiled, whereupon the mineralization mainly progressed thanks to the action of • OH adsorbed on the anode surface. Despite the incomplete mineralization using BDD as the anode, a remarkable toxicity decrease was determined. Fluoxetine degradation yielded F − and NO3 − ions, along with several aromatic intermediates. These included two chloroorganics, as a result of the anodic oxidation of Cl − to active chlorine. A detailed mechanism for the Fe(III)-EDDS-catalyzed PEF treatment of fluoxetine in urban wastewater is finally proposed.

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Section: Introductionmentioning

confidence: 99%

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

Brillas

Centellas

et al. 2020

Water Research

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“…Following this line, a recent work by Audino et al (2019) has proposed a kinetic study describing Fenton and photo-Fenton degradation of paracetamol in an annular photo-reactor, including the local volumetric rate of photon absorption effect. The work by Soriano-Molina et al (2018) proposed a mechanistic model of solar photo-Fenton.…”

Section: Introductionmentioning

confidence: 99%

A novel modeling approach for a generalizable photo-Fenton-based degradation of organic compounds

Audino

Pérez-Moya

Graells

et al. 2020

Environ Sci Pollut Res

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This work aims at proposing and validating a model that can be exploited for the future development of industrial applications (e.g., process design and control) of Fenton and photo-Fenton processes. Hence, a compromise modeling solution has been developed between the non-generalizable accuracy of the first principles models (FPMs) and the oversimplification of the empirical models (EMs). The work presents a novel model of moderate complexity that is simplified enough to be generalizable and computationally affordable, while retaining physical meaning. The methodology is based on a general degradation mechanism that can be algorithmically generated from the carbon number of the target compound, as well as from the knowledge of two kinetic parameters, one for the faster initial rate and the other one for the subsequent degradation steps. The contaminant degradation mechanism has been combined with an appropriately simplified implementation of the well-known Fenton and photo-Fenton kinetics. This model describes the degradation not only of the target compound and of the oxidant, but also of total organic carbon (TOC), which is used to define the overall quality of the water. Experimental design techniques were used along with a non-conventional modeling methodology of programmable process structures (PPS). This novel modeling approach was applied and validated on the degradation of three model compounds. A successful prediction of the evolution of the contaminants H 2 O 2 and TOC was confirmed and assessed by the root mean square error (RMSE).

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“…In particular, ethylenediamine-N,N'-disuccinic (EDDS) acid has been employed to form the Fe(III)-EDDS complex and catalyze the conventional Fenton-based processes. The performance of this aminopolycarboxylic acid (APCA) has only been tested in non-electrochemical Fenton-like systems, both in the dark [27] and under UV [28] or sunlight irradiation [29]. An electrochemical approach could enhance the continuous electroreduction of Fe(III)-EDDS complex from reaction (3), thus giving rise to a new kind of homogeneous EF process.…”

Section: Introductionmentioning

confidence: 99%

Electro-Fenton process at mild pH using Fe(III)-EDDS as soluble catalyst and carbon felt as cathode

Brillas

Centellas

et al. 2019

Applied Catalysis B: Environmental

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The feasibility of destruction of organic pollutants in water at near-neutral pH by homogeneous electro-Fenton (EF) process employing a soluble Fe(III)-EDDS complex as catalyst is demonstrated for the first time. The performance of the Fe(III)-EDDS-assisted EF process with carbon-felt or air-diffusion cathodes was evaluated from the degradation of butylated hydroxyanisole (BHA) in sulfate medium. The influence of applied current, pH and Fe(III):EDDS ratio and dosage on BHA decay and mineralization was related to the evolution of H2O2 and iron concentrations. Using Fe(III)-EDDS, up to 50% Fe(II) regeneration was achieved in 10 min, whereas only 23% was transformed using hydrated Fe 3+ . Almost total removal of BHA was achieved thanks to homogenous Fenton, heterogeneous Fenton with cathodically adsorbed Fe(III), and electrocatalysis. The mineralization partly corresponded to the gradual destruction of EDDS by hydroxyl radical (kabs = 5.22×10 9 M -1 s -1 ), and involved the formation of 5 oxidation and 6 dimerization or cyclization by-products.

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Mechanistic modeling of solar photo-Fenton process with Fe3+-EDDS at neutral pH

Cited by 56 publications

References 45 publications

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

Expanding the application of photoelectro-Fenton treatment to urban wastewater using the Fe(III)-EDDS complex

A novel modeling approach for a generalizable photo-Fenton-based degradation of organic compounds

Electro-Fenton process at mild pH using Fe(III)-EDDS as soluble catalyst and carbon felt as cathode

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